Designing broadband pulsed dynamic nuclear polarization sequences in static solids

Dynamic nuclear polarization (DNP) is a nuclear magnetic resonance (NMR) hyperpolarization technique that mediates polarization transfer from unpaired electrons with large thermal polarization to NMR-active nuclei via microwave (mw) irradiation. The ability to generate arbitrarily shaped mw pulses using arbitrary waveform generators allows for remarkable improvement of the robustness and versatility of DNP. We present here novel design principles based on single-spin vector effective Hamiltonian theory to develop new broadband DNP pulse sequences, namely, an adiabatic version of XiX (X-inverse X)-DNP and a broadband excitation by amplitude modulation (BEAM)-DNP experiment. We demonstrate that the adiabatic BEAM-DNP pulse sequence may achieve a H-1 enhancement factor of similar to 360, which is better than ramped-amplitude NOVEL (nuclear spin orientation via electron spin locking) at similar to 0.35 T and 80 K in static solids doped with trityl radicals. In addition, the bandwidth of the BEAM-DNP experiments (similar to 50 MHz) is about three times the H-1 Larmor frequency. The generality of our theoretical approach will be helpful in the development of new pulsed DNP sequences.

Automated summary

Dynamic nuclear polarization (DNP) is a technique that transfers thermal polarization from unpaired electrons to NMR-active nuclei via microwave irradiation. This study presents novel design principles based on single-spin vector effective Hamiltonian theory for developing new broadband DNP pulse sequences and demonstrates their effectiveness.